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A pyrocarbonate intermediate for CO2 activation and selective conversion in bifunctional metal-organic frameworks
- An, Bing, Meng, Yaping, Li, Zhe, Hong, Yahui, Wang, Tingting, Wang, Shuai, Lin, Jingdong, Wang, Cheng, Wan, Shaolong, Wang, Yong, Lin, Wenbin
- Journal of catalysis 2019 v.373 pp. 37-47
- carbon dioxide, catalysts, catalytic activity, coordination polymers, esterification, formates, hydrogenation, nanoparticles, palladium, value-added products
- CO2 activation and conversion are of significant interest. Here we report a mono-alkyl pyrocarbonate-bipyridinium salt intermediate to activate CO2 for synthesizing ethyl formate as a value-added product via tandem esterification and hydrogenation. The required basic bipyridine sites for CO2 activation and metallic Pd nanoparticles for hydrogenation were assembled in the same nano-cavity of a designer metal–organic framework (MOF). This MOF hybrid exhibits a high catalytic activity to generate ethyl formate (HCO2Et) (1333 μmol/gcat/h) with 93.5% selectivity at 412 K. The turnover frequency of HCO2Et based on the number of exposed Pd atoms is up to 22.2 h−1, higher than those of other catalysts previously reported for generating alkyl formates from CO2 under similar conditions.